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Errors in nanoparticle growth rates inferred from measurements in chemically reacting aerosol systems

机译:从化学反应气溶胶系统的测量中推断纳米粒子生长率的误差

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In systems in which aerosols are being formed by chemical transformations, individual particles grow due to the addition of molecular species. Efforts to improve our understanding of particle growth often focus on attempts to reconcile observed growth rates with values calculated from models. However, because it is typically not possible to measure the growth rates of individual particles in chemically reacting systems, they must be inferred from measurements of aerosol properties such as size distributions, particle number concentrations, etc. This work discusses errors in growth rates obtained using methods that are commonly employed for analyzing atmospheric data. We analyze “data” obtained by simulating the formation of aerosols in a system in which a single chemical species is formed at a constant rate, R. We show that the maximum overestimation error in measured growth rates occurs for collision-controlled nucleation in a single-component system in the absence of a preexisting aerosol, wall losses, evaporation or dilution, as this leads to the highest concentrations of nucleated particles. Those high concentrations lead to high coagulation rates that cause the nucleation mode to grow faster than would be caused by vapor condensation alone. We also show that preexisting particles, when coupled with evaporation, can significantly decrease the concentration of nucleated particles. This can lead to decreased discrepancies between measured growth rate and true growth rate by reducing coagulation among nucleated particles. However, as particle sink processes become stronger, measured growth rates can potentially be lower than true particle growth rates. We briefly discuss nucleation scenarios in which the observed growth rate approaches zero while the true growth rate does not.
机译:在通过化学转化形成气溶胶的系统中,各个颗粒由于添加分子种而生长。提高我们对粒子增长的理解的努力通常集中在试图与由模型计算的价值进行重新调和的生长速率。然而,因为通常不可能测量化学反应系统中单个颗粒的生长速率,因此必须从诸如尺寸分布,粒子数浓度等的气溶胶性质的测量推断它们。该工作讨论了使用的生长速率的误差通常用于分析大气数据的方法。我们分析通过模拟形成单个化学物质以恒定速率形成的系统中的气溶胶形成而获得的“数据”。我们表明,在单个碰撞控制的成核中,测量的生长速率的最大高估误差发生 - 在没有预先存在的气溶胶,壁损失,蒸发或稀释的情况下的组合系统,因为这导致最高浓度的核心颗粒。那些高浓度导致高凝血率,导致成核模式生长得比单独的蒸汽凝结引起的速度快。我们还表明,当与蒸发结合时,预先存在的颗粒可以显着降低核化颗粒的浓度。这可能导致通过减少核颗粒中的凝血来降低测量的生长速率和真正的增长率之间的差异。然而,随着粒子水槽过程变得更强,测量的生长速率可能低于真正的颗粒生长速率。我们简要讨论了核心情景,其中观察到的增长率达到零,而真正的增长率则没有。

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